Unraveling oxygen vacancy-driven catalytic selectivity and hot electron generation on heterointerfaces using nanostructured platform

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: March 25, 2025

Modulating the physicochemical properties of oxides is crucial to achieve efficient and desirable reactions in heterogeneous catalysis. However, their catalytic role not clearly identified because unevenly distributed interfaces close conjugation with metal catalysts may hinder distinguishing contribution complex random structures. Here, we demonstrate a model platform composed well-aligned CeOx nanowire arrays on Pt observe systematically. Independently modulating crystallinity oxygen vacancy concentration oxide nanowires, while preserving interfaces, enables quantitative analysis individual effects partial oxidation selectivity, resulting hot electron generation during methanol reactions. treated vacuum annealing exhibits 1.47- 2.12-times higher selectivity methyl formate chemicurrent yield than without Pt. Density-functional theory calculations reveal that promoted charge transfer from electron-accumulated interface driven by acts as key parameter enhancing selectivity. Tuning essential for achieving selective catalysis, yet precise remains unclear. authors present featuring catalysts, enabling systematic investigation function.

Language: Английский

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Is the ∗O vs. ∗OH scaling relation intercept more relevant than the ∗OOH vs. ∗OH intercept to capture trends in the oxygen evolution reaction?

Chem Catalysis, Journal Year: 2024, Volume and Issue: 4(7), P. 101039 - 101039

Published: July 1, 2024

The transition from fossil fuels to renewable energy sources is inevitable, and electrocatalytic water splitting produce hydrogen one of the core processes that must be further optimized. Regrettably, anodic oxygen evolution reaction (OER) severely limits its efficiency. Theory explains humble intrinsic activity OER catalysts by scaling relations between intermediates. While relation ∗OOH ∗OH intermediates well established, only slope ∗O vs.∗OH has an estimated numerical value, whereas intercept this frequently assumed zero. Herein, we demonstrate how deviations assumption cause changes in shape volcano plot prevalent mechanisms at apex plot. Our derived plots may enable progress design shifting focus on vs. relation.

Language: Английский

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The application and research progress of d-band center theory in the field of water electrolysis

International Journal of Hydrogen Energy, Journal Year: 2025, Volume and Issue: 132, P. 183 - 211

Published: May 1, 2025

Language: Английский

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Addressing the Complexity of Bridging Thermal and Reactive Catalysis. The Role of Strong Localised Electrical Fields

Topics in Catalysis, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 3, 2025

Language: Английский

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Electrocatalysis: Prospects and Role to Enable an E‐Chemistry Future

The Chemical Record, Journal Year: 2025, Volume and Issue: unknown

Published: March 3, 2025

Abstract Electrocatalysis is a crucial technology that will enable future low‐carbon chemical production and energy beyond fossil fuels. Notwithstanding the intense growing research in area, potentialities of field are largely unexplored. We provide case examples discuss emerging possibilities have still not been investigated enough but necessary to exploit this potential e‐chemistry. Starting from defining trends setting scene, as well clarifying difference between electrochemistry electrocatalysis, some elements vision foster innovation discussed. The aim stimulate discussion reflection rather than review state‐of‐the‐art. Aspects discussed regard i) passing electro photoelectrocatalytic approaches, ii) making chemicals air, iii) exploitation both anodic cathodic reactions, tandem/paired electrocatalytic iv) for selective oxidation mediated synthesis. Priorities strategies an e‐chemistry Intensifying these directions extending still‐too‐limited current including modelling design, effort accelerate realisation distributed

Language: Английский

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Trends in the oxygen adsorption energy derived from the thermodynamic potential model for the oxygen evolution reaction

Catalysis Today, Journal Year: 2024, Volume and Issue: 443, P. 114963 - 114963

Published: July 29, 2024

Across the last years, substantial efforts were done to understand limitations of oxygen evolution reaction (OER) catalysts and develop robust ones such as solve efficiency problem in water splitting. Fundamental understanding represents a pathway towards designing superior catalysts. In this direction, several descriptors (ηTD, ESSI, Gmax(η)) have been derived based on adsorption energies OER intermediate moieties (∆EHO*/∆EO*/∆EHOO*) for faster screening materials. A universal scaling between HO* HOO* was established wide range materials many cases shown govern minimum theoretical overpotential. On other hand, O* fragments large scattering along trendline. work we derive five trends overpotential intervals, using data collected from published studies employing DFT calculations OER. It is that best an energy placed within limited interval, yet sufficiently pool promising (-0.5,1.5 eV), scales with at slope one intercept 1.81 eV. Furthermore, decrease 3.14 (valid all analyzed) 3.03 eV found. For three four trends, O*/HO*scaling intercepts closer either (2.2/2.78) or HO*(1.43/0.78) energies. each set data, varies 3 3.37 Separately, analyzed TiO2(110) semiconducting rutile surface when doped transition metals modified (i) H* co-adsorbed act charge donor/acceptor (ii) provided excess lack electrons. The analysis performed literature, supplemented by additional calculations. Clear amount obtained standard GGA functionals used. An origin variation systems similar HO*/HOO* provided. However, Hubbard corrected functional used, some change. Clearly, it still challenge describing accurately cost-effective manner undoped metal oxides, especially O*. strategy get further insight into variations discussed.

Language: Английский

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Unraveling the competition between the oxygen and chlorine evolution reactions in seawater electrolysis: Enhancing selectivity for green hydrogen production

Electrochimica Acta, Journal Year: 2024, Volume and Issue: 497, P. 144534 - 144534

Published: June 6, 2024

Language: Английский

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Enhancing catalytic performance and hot electron generation through engineering metal-oxide and oxide-oxide interfaces

Catalysis Today, Journal Year: 2023, Volume and Issue: 425, P. 114306 - 114306

Published: Aug. 1, 2023

Language: Английский

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Theoretical advances in understanding the active site microenvironment toward the electrocatalytic nitrogen reduction reaction in aqueous media

Current Opinion in Electrochemistry, Journal Year: 2023, Volume and Issue: 42, P. 101383 - 101383

Published: Aug. 30, 2023

The electrocatalytic nitrogen reduction reaction (eNRR) in aqueous media has received substantial attention because it enables the direct conversion of N2 to NH3 under benign conditions. There are, however, many factors limiting overall eNRR efficiency, including competing hydrogen evolution (HER) and sluggish kinetics due a strong N≡N bond. These challenges call for more systematic theoretical insight into mechanism guide rational optimization experimental designs. In this review, we present latest computational advances an medium, key aspects both catalyst design proton accessibility. Specifically, discuss importance constant potential explicit solvent simulations, role electrochemical interface, impact active center microenvironment on activity selectivity. Finally, current future prospects are addressed.

Language: Английский

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Enhancement of nitrogen reduction reaction activity of sp-B-doped γ-graphyne nanotubes through curvature effect

Molecular Catalysis, Journal Year: 2024, Volume and Issue: 558, P. 114044 - 114044

Published: March 16, 2024

Language: Английский

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